Electrocatalytic CO_(2)reduction into CO has been regarded as one of the most promising strategies for sustainable carbon cycles at ambient conditions,but still faces challenges to achieve both high product selectivit...Electrocatalytic CO_(2)reduction into CO has been regarded as one of the most promising strategies for sustainable carbon cycles at ambient conditions,but still faces challenges to achieve both high product selectivity and large current density.Here,we report a Ni_(4)N/Ni_(3)ZnC_(0.7)heterostructured electrocatalyst embedded in accordion-like N-doped carbon through a simple molten salt annealing strategy.The optimal Ni_(4)N/Ni_(3)ZnC_(0.7)electrocatalyst achieves a high CO Faraday efficiency of 92.3%and a large total current density of-15.8 m A cm^(-2)at-0.8 V versus reversible hydrogen electrode,together with a long-term stability about 30 h.Density functional theory results reveal that the energy barrier for*COOH intermediate formation largely decreased on Ni_(4)N/Ni_(3)ZnC_(0.7)heterostructure compared with Ni_(4)N and Ni_(3)ZnC_(0.7),thus giving rise to enhanced activity and selectivity.A rechargeable Zn-CO_(2)battery is further assembled with Ni_(4)N/Ni_(3)ZnC_(0.7)catalyst as the cathode,which shows a maximum power density of 0.85 mW cm^(-2)and excellent stability.展开更多
基金financially supported by the National Key Research and Development Program,China(2018YFB1502503)the 2021 Talent Introduction Project of Chongqing Medical and Pharmaceutical College(ygz2021104)。
文摘Electrocatalytic CO_(2)reduction into CO has been regarded as one of the most promising strategies for sustainable carbon cycles at ambient conditions,but still faces challenges to achieve both high product selectivity and large current density.Here,we report a Ni_(4)N/Ni_(3)ZnC_(0.7)heterostructured electrocatalyst embedded in accordion-like N-doped carbon through a simple molten salt annealing strategy.The optimal Ni_(4)N/Ni_(3)ZnC_(0.7)electrocatalyst achieves a high CO Faraday efficiency of 92.3%and a large total current density of-15.8 m A cm^(-2)at-0.8 V versus reversible hydrogen electrode,together with a long-term stability about 30 h.Density functional theory results reveal that the energy barrier for*COOH intermediate formation largely decreased on Ni_(4)N/Ni_(3)ZnC_(0.7)heterostructure compared with Ni_(4)N and Ni_(3)ZnC_(0.7),thus giving rise to enhanced activity and selectivity.A rechargeable Zn-CO_(2)battery is further assembled with Ni_(4)N/Ni_(3)ZnC_(0.7)catalyst as the cathode,which shows a maximum power density of 0.85 mW cm^(-2)and excellent stability.